In this chapter, a summary of the recent progress on the incorporation of graphitic carbon-based nanomaterials, such as graphene particles and CNTs, in composites to develop multifunctional materials with remarkable mechanical performance is presented. Among the functionalities discussed in this chapter are self-sensing (damage detection), self-healing, and actuation. Most of the research proposed in this chapter is yet in the research and development stage, and the utilization of those materials in industrial scales requires further material property optimization and development of more economic production techniques.